Litcius/Paper detail

Zn-Nx sites on N-doped carbon for aerobic oxidative cleavage and esterification of C(CO)-C bonds

Chao Xie, Longfei Lin, Liang Huang, Zixin Wang, Zhiwei Jiang, Zehui Zhang, Buxing Han

2021Nature Communications190 citationsDOIOpen Access PDF

Abstract

Abstract Selective cleavage of C-C bonds is very important in organic chemistry, but remains challenging because of their inert chemical nature. Herein, we report that Zn/NC-X catalysts, in which Zn 2+ coordinate with N species on microporous N-doped carbon (NC) and X denotes the pyrolysis temperature, can effectively catalyze aerobic oxidative cleavage of C(CO)-C bonds and quantitatively convert acetophenone to methyl benzoate with a yield of 99% at 100 °C. The Zn/NC-950 can be applied for a wide scope of acetophenone derivatives as well as more challenging alkyl ketones. Detail mechanistic investigations reveal that the catalytic performance of Zn/NC-950 can be attributed to the coordination between Zn 2+ and N species to change the electronic state of the metal, synergetic effect of the Zn single sites with their surrounding N atoms, as well as the microporous structure with the high surface area and structural defects of the NC.

Topics & Concepts

Microporous materialCatalysisChemistryAcetophenonePyrolysisAlkylBond cleavageOrganometallic chemistryCarbon fibersCleavage (geology)Organic chemistryMaterials scienceFracture (geology)Composite materialComposite numberCatalytic Processes in Materials ScienceCovalent Organic Framework ApplicationsAdvanced Photocatalysis Techniques